Abstract
Learning to engineer self-assembly would enable the precise organization of molecules by design to create matter with tailored properties. Here we demonstrate that proteins can direct the self-assembly of buckminsterfullerene (C60) into ordered superstructures. A previously engineered tetrameric helical bundle binds C60 in solution, rendering it water soluble. Two tetramers associate with one C60, promoting further organization revealed in a 1.67-Å crystal structure. Fullerene groups occupy periodic lattice sites, sandwiched between two Tyr residues from adjacent tetramers. Strikingly, the assembly exhibits high charge conductance, whereas both the protein-alone crystal and amorphous C60 are electrically insulating. The affinity of C60 for its crystal-binding site is estimated to be in the nanomolar range, with lattices of known protein crystals geometrically compatible with incorporating the motif. Taken together, these findings suggest a new means of organizing fullerene molecules into a rich variety of lattices to generate new properties by design.
Highlights
Learning to engineer self-assembly would enable the precise organization of molecules by design to create matter with tailored properties
By learning to engineer the assembly of these molecules, myriad other molecular building blocks can be coorganized in desired ways through non-covalent or covalent attachment
We closely investigate the interfacial geometry of the C60-binding motif, finding it to be common among protein crystal lattices
Summary
Learning to engineer self-assembly would enable the precise organization of molecules by design to create matter with tailored properties. The affinity of C60 for its crystal-binding site is estimated to be in the nanomolar range, with lattices of known protein crystals geometrically compatible with incorporating the motif. Taken together, these findings suggest a new means of organizing fullerene molecules into a rich variety of lattices to generate new properties by design. It has been a daunting challenge to quantitatively describe and control the driving forces that govern self-assembly, given the broad range of molecular building blocks one would like to organize. This, together with the simple (and naturally recurrent) geometry of the C60-binding motif we discover, suggests that it may be possible to use the structural principles emergent from our study to generate a variety of C60–protein co-assemblies to further explore and exploit the properties of fullerenes[26]
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